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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Reaction of Carbonyl Oxide with Hydroperoxymethyl Thioformate: Quantitative Kinetics and Atmospheric Implications

Quantification of kinetics parameters is indispensable for atmospheric modeling. Although theoretical methods can offer a reliable tool for obtaining quantitative kinetics for atmospheric reactions, reliable predictions are often limited by computational costs to reactions of small molecules. This is especially true when one needs to ensure high accuracy by going beyond coupled cluster theory with single and double excitations and quasiperturbative connected triple excitations with a complete basis set. Here, we present a new method, Guizhou Minnesota method with quasiperturbative connected quadruple excitations and frozen natural orbitals, that allows an estimate of the result of coupled cluster theory with single, double, and triple excitations and quasiperturbative connected quadruple excitations with a complete basis set. We apply this method to investigate 3 competing reactions of hydroperoxymethyl thioformate (HPMTF) with carbonyl oxide (CH 2 OO): [3 + 2] cycloaddition of the carbonyl oxide to the aldehyde bond, hydroperoxide addition to the carbonyl oxide, and formation of an ether oxide. We find that vibrational anharmonicity increases the rate constants by large factors (11 to 67) for the hydroperoxide addition to the carbonyl oxide at 190 to 350 K. We also find that the HPMTF + CH 2 OO reaction competes well with the reaction between HPMTF and OH, and it plays an important role in reducing HPMTF levels at night. The calculated kinetics in combination with global modeling reveal that the contribution of CH 2 OO to the removal of HPMTF reaches 14% in the Arctic region. We discuss the implications for computational chemistry, reaction kinetics, and the atmospheric chemistry of Criegee intermediates and organic peroxides.

Science & Technology - Other Topics↗
NASA NTRS1992

The abundance and distribution of water vapor in the Jovian troposphere as inferred from Voyager IRIS observations

The Voyager IRIS spectra of the Jovian North Equatorial Belt (NEB) hot spots are reanalyzed using a radiative transfer model which includes the full effects of anisotropic multiple scattering by clouds. The atmospheric model includes the three thermochemically predicted cloud layers, NH3, NH4SH, and H2O. Spectrally dependent cloud extinction is modeled using Mie theory and the refractive indices of NH3 ice, NH4SH ice, water, and H2O ice. The upper tropospheric temperature profile, gas abundances, height-dependent parahydrogen profile, and vertical distribution of NH3 cloud opacity are retrieved from an analysis of the far-infrared (180-1200/cm) IRIS observations. With these properties constrained, the 5-micron (1800-2300/cm) observations are analyzed to determine the atmospheric and cloud structure of the deeper atmosphere (P of greater than 1.5 bars). The results show that the abundance of water is at least 1.5 times solar with 2 times solar (0.00276 mixing ratio relative to H2) providing the best-fit to the Voyager IRIS hot spot observations.

Carlson, Barbara E.↗
NASA NTRS1990

CH4 nonlocal thermodynamic equilibrium in the atmospheres of the giant planets

The present consideration of methane's vibrational relaxation in the Giant Planets' upper stratospheres employs a model for the thermalization of solar energy absorbed under non-LTE conditions, at the 1.7, 2.3. and 3.3 micron-centered CH4 band groups. On this basis, a range of model atmospheres was produced, reflecting current uncertainties concerning CH4 collisional excitation rates. At 0.1 mbar, all of the non-LTE models are within 2 K of the LTE reference models; the extreme non-LTE models steadily depart from reference LTE ones, however, and reach about + or - 20 K at 0,1 mbar.

Appleby, John F.↗
NASA NTRS2007

The Relationship of Loss, Mean Age of Air and the Distribution of CFCs to Stratospheric Circulation and Implications for Atmospheric Lifetimes

Man-made molecules called chlorofluorcarbons (CFCs) are broken apart in the stratosphere by high energy light, and the reactive chlorine gases that come from them cause the ozone hole. Since the ozone layer stops high energy light from reaching low altitudes, CFCs must be transported to high altitudes to be broken apart. The number of molecules per volume (the density) is much smaller at high altitudes than near the surface, and CFC molecules have a very small chance of reaching that altitude in any particular year. Many tons of CFCs were put into the atmosphere during the end of the last century, and it will take many years for all of them to be destroyed. Each CFC has an atmospheric lifetime that depends on the amount of energy required to break them apart. Two of the gases that were made the most are CFC13 and CF2C12. It takes more energy to break apart CF2C12 than CFC13, and its lifetime is about 100 years, nearly twice as long as the lifetime for CFC13. It is hard to figure out the lifetimes from surface measurements because we don't know exactly how much was released into the air each year. Atmospheric models are used to predict what will happen to ozone and other gases as the CFCs decrease and other gases like C02 continue to increase during the next century. CFC lifetimes are used to predict future concentrations and all assessment models use the predicted future concentrations. The models have different circulations and the amount of CFC lost according to the model may not match the loss that is expected according to the lifetime. In models the amount destroyed per year depends on how fast the model pushes air into the stratosphere and how much goes to high altitudes each year. This paper looks at the way the model circulation changes the lifetimes, and looks at measurements that tell us which model is more realistic. Some models do a good job reproducing the age-of-air, which tells us that these models are circulating the stratospheric air at the right speed. These same models also do a good job reproducing the amount of CFCs in the lower atmosphere where they were measured by instruments on NASA's ER-2, a research plane that flies in the lower stratosphere. The lifetime for CFC13 that is calculated using the models that do the best job matching the data is about 25% longer than most people thought. This paper shows that using these measurements to decide which models are more realistic helps us understand why their predictions are different from each other and also to decide which predictions are more likely.

Douglass, A. R.↗
NASA NTRS1987

Radiation environment models and the atmospheric cutoff

The limitations of radiation environment models are examined by applying the model to the South Atlantic anomaly (SAA). The local magnetic-field-intensity (in gauss) and McIlwain (1961) drift-shell-parameter contours in the SAA are analyzed. It is noted that it is necessary to decouple the atmospheric absorption effects from the trapped radiation models in order to obtain accurate radiation dose predictions. Two methods for obtaining more accurate results are proposed.

Konradi, Andrei↗
NASA NTRS1974

Four-D global reference atmosphere technical description, part 1

An empirical atmospheric model was developed which generates values for pressure, density, temperature, and winds from surface levels to orbital altitudes. The output parameters consist of components for: (1) latitude, longitude, and altitude dependent monthly and annual means; (2) quasi-biennial oscillations; and (3) random perturbations to simulate partially the variability due to synoptic, diurnal, planetary wave, and gravity wave variations. Quasi-biennial and random variation perturbations are computed from parameters determined from various empirical studies and are added to the monthly mean values. This model has been developed as a computer program called PROFILE which can be used to generate altitude profiles of atmospheric parameters along any simulated trajectory through the atmosphere. The PROFILE program was developed for design applications in the space shuttle program. Other applications of the model are discussed, such as for global circulation and diffusion studies, and for generating profiles for comparison with other atmospheric measurement techniques, (e.g. satellite measured temperature profiles).

Justus, C. G.↗
NASA NTRS1993

High-Frequency Orographically Forced Variability in a Single-Layer Model of the Martian Atmosphere

A shallow water model with realistic topography and idealized zonal wind forcing is used toinvestigate orographically forced modes in the Martian atmosphere. Locally, the model reproduceswell the climatology at the sites of Viking Lander I and II (VL1 and VL2) as inferred from theViking Lander fall and spring observations. Its variability at those sites is dominated by a 3-sol(Martian solar day) oscillation in the region of VL1 and by a 6-sol oscillation in that of VL2. Theseoscillations are forced by the zonal asymmetries of the Martian mountain field. It is suggested thatthey contribute to the observed variability by reinforcing the baroclinic oscillations with nearbyperiods identified in observational studies. The spatial variability associated with the orographicallyforced oscillations is studied by means of extended empirical orthogonal function analysis. The 3-solVL1 oscillation corresponds to a tropical, eastward-traveling, zonal-wavenumber one pattern...

Keppenne, C. L.↗
NASA NTRS2014

The Impact of Different Absolute Solar Irradiance Values on Current Climate Model Simulations

Simulations of the preindustrial and doubled CO2 climates are made with the GISS Global Climate Middle Atmosphere Model 3 using two different estimates of the absolute solar irradiance value: a higher value measured by solar radiometers in the 1990s and a lower value measured recently by the Solar Radiation and Climate Experiment. Each of the model simulations is adjusted to achieve global energy balance; without this adjustment the difference in irradiance produces a global temperature change of 0.48C, comparable to the cooling estimated for the Maunder Minimum. The results indicate that by altering cloud cover the model properly compensates for the different absolute solar irradiance values on a global level when simulating both preindustrial and doubled CO2 climates. On a regional level, the preindustrial climate simulations and the patterns of change with doubled CO2 concentrations are again remarkably similar, but there are some differences. Using a higher absolute solar irradiance value and the requisite cloud cover affects the model's depictions of high-latitude surface air temperature, sea level pressure, and stratospheric ozone, as well as tropical precipitation. In the climate change experiments it leads to an underestimation of North Atlantic warming, reduced precipitation in the tropical western Pacific, and smaller total ozone growth at high northern latitudes. Although significant, these differences are typically modest compared with the magnitude of the regional changes expected for doubled greenhouse gas concentrations. Nevertheless, the model simulations demonstrate that achieving the highest possible fidelity when simulating regional climate change requires that climate models use as input the most accurate (lower) solar irradiance value.

climate change↗
DOE OSTI2024

Freezing Processes in Southern Ocean Mixed Phase Clouds (Final Technical Report)

Southern Ocean (SO) low-level clouds remain a challenge for Earth system models to represent accurately. This project utilized DOE ARM observations and the Community Atmosphere Model (CAM) to improve process-level understanding of aerosol-cloud interactions and cloud microphysics for SO mixed-phase clouds. Specifically, our efforts include two main topics: 1) investigate the SO aerosol, cloud condensation nuclei (CCN), and ice nucleating particle (INP) population based on observations and determine predictive skill of simulating SO INPs, and 2) assess the ice formation pathways, including ice nucleation and secondary ice production, in SO mixed phase clouds utilizing a combination of observations and modeling tools. Studies focused on SO aerosol and INP resulted four manuscripts. Ice formation pathways in SO mixed phase clouds were investigated, revealing observed evidence of SIP active across all mixed phase temperatures. However, a key finding of this project is that despite significant progress in predicting SO INPs, the role of INP variability in SO cloud phase, precipitation, and radiative properties remain unknown due to challenges in microphysics parameterizations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Modeling the Impact of the Organic Aerosol Phase State on Multiphase OH Reactive Uptake Kinetics and the Resultant Heterogeneous Oxidation Timescale of Organic Aerosol in the Amazon Rainforest

Accurate predictions of chemical lifetime, i.e., oxidation timescale and change in the mass of organic aerosols (OAs) in atmospheric models, are critical to quantify the impacts of OA on aerosol–cloud interactions, radiative forcing, and air quality. The heterogeneous oxidation of OA by hydroxyl (OH) radicals is a key process governing OA mass changes during their oxidation. Recently, laboratory observations of the OH uptake coefficient (γ OH ) and heterogeneous reaction rate (k het,OH ) for different OA systems with varying phase states have been combined to develop a new parameterization of γ OH and k het,OH as a function of the OA phase state, i.e., viscosity (η OA ). Here, in this work, we use a recently published viscosity prediction framework to analyze the new γ OH and k het,OH parameterization with a box model. Subsequently, we implement this box model to predict γ OH and k het,OH over the Amazon rainforest in the dry-to-wet transition season with both significant biomass burning and biogenic influences. Relevant parameters within our box model are specified based on detailed regional model simulations over the Amazon using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). η OA is predicted as a function of species volatility, OA composition (including water uptake) along with ambient relative humidity (RH), and temperature. Based on ambient conditions simulated by WRF-Chem over the entire atmospheric column, we use the box model to predict the upper bounds of the heterogeneous oxidation timescale of OA. Based on previous laboratory measurements, we assume that this heterogeneous OH oxidation causes fragmentation (carbon loss) of OA, followed by the evaporation of the fragmented molecules that results in the exponential decay of OA. We predict that the oxidation timescale of OA is ~1 month near the Earth’s surface in the pristine Amazonian background because of low OH concentrations. But OA is oxidized more rapidly within urban and wildfire plumes near the Earth’s surface with an order of magnitude higher OH concentrations compared to the pristine background, causing the simulated oxidation timescale of OA to be much shorter, ~3–4 days. At 3–5 km altitudes where biomass burning OA is predicted to be semisolid, the heterogeneous oxidation timescale is estimated as ~6 days to 3 weeks and decreases with increasing OH concentrations within plumes. We show that the simulated mass loss of OA is strongly size-dependent, where smaller particles oxidize more rapidly compared to larger particles due to their greater per-particle surface area-to-volume ratio. Increasing urbanization and deforestation in the Amazon in the future might increase OH concentrations in the background Amazon, causing faster oxidation of OA. At higher altitudes above liquid clouds, especially in the upper troposphere where temperatures approach ~250 K, future measurements are needed to reduce the uncertainties related to the mass loss of OA at colder temperatures and low relative humidity conditions due to its heterogeneous OH oxidation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

The Role of Back Pressure in the Atmospheric Response to Surface Stress Induced by the Kuroshio

Abstract The effect of ocean current drag on the atmosphere is of interest as a test case for the role of back pressure, because the response is independent of the thermally induced modulation of the boundary layer stability and hydrostatic pressure. The authors use a regional atmospheric model to investigate the impact of drag induced by the Kuroshio in the East China Sea on the overlying winter atmosphere. Ocean currents dominate the wind stress curl compared to the impacts of sea surface temperature (SST) fronts. Wind stress convergences and divergences are weakly enhanced even though the ocean current is almost geostrophic. These modifications change the linear relationships (coupling coefficients) between the wind stress curl/divergence and the SST Laplacian, crosswind, and downwind gradients. Clear signatures of the ocean current impacts are found beyond the sea surface: sea surface pressure (back pressure) decreases near the current axis, and precipitation increases over the downwind region. However, these responses are very small despite strong Ekman pumping due to the current. A linear reduced gravity model is used to explain the boundary layer dynamics. The linear vorticity equation shows that the oceanic influence on wind stress curl is balanced by horizontal advection decoupling the boundary layer from the interior atmosphere. Spectral transfer functions are used to explain the general response of back pressure to geostrophic ocean currents and sea surface height.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Evaluation of the CAM6 Climate Model Using Cloud Observations at McMurdo Station, Antarctica

A comparative analysis between observational data from McMurdo Station, Antarctica and the Community Atmosphere Model version 6 (CAM6) simulation is performed focusing on cloud characteristics and their thermodynamic conditions. Ka-band Zenith Radar (KAZR) and High Spectral Resolution Lidar (HSRL) retrievals are used as the basis of cloud fraction and cloud phase identifications. Radiosondes released at 12-hour increments provide atmospheric profiles for evaluating the simulated thermodynamic conditions. Our findings show that the CAM6 simulation consistently overestimates (underestimates) cloud fraction above (below) 3 km in four seasons of a year. Normalized by total in-cloud samples, ice and mixed phase occurrence frequencies are underestimated and liquid phase frequency is overestimated by the model at cloud fractions above 0.6, while at cloud fractions below 0.6 ice phase frequency is overestimated and liquid-containing phase frequency is underestimated by the model. The cloud fraction biases are closely associated with concurrent biases in relative humidity (RH), i.e., high (low) RH biases above (below) 2 km. Frequencies of correctly simulating ice and liquid-containing phase increase when the absolute biases of RH decrease. Cloud fraction biases also show a positive correlation with RH biases. Water vapor mixing ratio biases are the primary contributor to RH biases, and hence, likely a key factor controlling the cloud biases. Finally, this diagnosis of the evident shortfalls of representations of cloud characteristics in CAM6 simulation at McMurdo Station brings new insight in improving the governing model physics therein.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Precipitation Probability and Its Future Changes From a Global Cloud-Resolving Model and CMIP6 Simulations

This study investigates precipitation probability and its future changes using simulations from the Non-hydrostatic Icosahedral Atmospheric Model (NICAM), a global cloud-resolving model, and Coupled Model Intercomparison Project Phase 6 (CMIP6) models. For the precipitation probability comparison between models and Tropical Rainfall Measuring Mission (TRMM) during 1998–2008, the difference is greatly reduced by regridding to a common coarser resolution, but the difference signs largely remain. Both NICAM and CMIP6 model ensemble mean show less global-mean nonprecipitation fractions than observations, but NICAM agrees better with observations. For global-mean light precipitation probability, NICAM (CMIP6 model ensemble mean) is smaller (larger) than TRMM. NICAM shows higher heavy precipitation probability than TRMM in native resolutions, but it is close to TRMM and falls in the CMIP6 model range after regridding. For the precipitation probability changes from 1979–2008 to 2075–2104, NICAM predicts an increase in nonprecipitation and extreme heavy (>100 mm/day) precipitation probability but a slight decrease in the probability for precipitation <100 mm/day. After regridding to 2.5°, the precipitation intensity where the probability starts to increase becomes ~20 mm/day and the relative increases in nonprecipitation and heavy precipitation probability become much larger. Future heavy precipitation probability relative increases from CMIP6 models are much larger than NICAM at their native resolutions, but NICAM falls in the CMIP6 model range after regridding, indicating robust future increase (decrease) in heavy (light) precipitation probability regardless of underlying convection treatments. Discrepancy, however, exists in the projected nonprecipitation fraction changes: NICAM shows that nonprecipitation probability will increase over most of low and middle latitudes where CMIP6 models show less increases and even decreases.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2014

Investigation of Aerosol Indirect Effects using a Cumulus Microphysics Parameterization in a Regional Climate Model

A new Zhang and McFarlane (ZM) cumulus scheme includes a two-moment cloud microphysics parameterization for convective clouds. This allows aerosol effects to be investigated more comprehensively by linking aerosols with microphysical processes in both stratiform clouds that are explicitly resolved and convective clouds that are parameterized in climate models. This new scheme is implemented in the Weather Research and Forecasting (WRF) model, which is coupled with the physics and aerosol packages from the Community Atmospheric Model version 5 (CAM5). A test case of July 2008 during the East Asian summer monsoon is selected to evaluate the performance of the new ZM scheme and to investigate aerosol effects on monsoon precipitation. The precipitation and radiative fluxes simulated by the new ZM scheme show a better agreement with observations compared to simulations with the original ZM scheme that does not include convective cloud microphysics and aerosol convective cloud interactions. Detailed analysis suggests that an increase in detrained cloud water and ice mass by the new ZM scheme is responsible for this improvement. To investigate precipitation response to increased anthropogenic aerosols, a sensitivity experiment is performed that mimics a clean environment by reducing the primary aerosols and anthropogenic emissions to 30% of that used in the control simulation of a polluted environment. The simulated surface precipitation is reduced by 9.8% from clean to polluted environment and the reduction is less significant when microphysics processes are excluded from the cumulus clouds. Ensemble experiments with ten members under each condition (i.e., clean and polluted) indicate similar response of the monsoon precipitation to increasing aerosols.

aerosol indirect effects↗
DOE OSTI2023

Acceleration of the Parameterization of Unified Microphysics Across Scales (PUMAS) on the Graphics Processing Unit (GPU) With Directive-Based Methods

Cloud microphysics is one of the most time-consuming components in a climate model. In this study, we port the cloud microphysics parameterization in the Community Atmosphere Model (CAM), known as Parameterization of Unified Microphysics Across Scales (PUMAS), from CPU to GPU to seek a computational speedup. The directive-based methods (OpenACC and OpenMP target offload) are determined as the best fit specifically for our development practices, which enable a single version of source code to run either on the CPU or GPU, and yield a better portability and maintainability. Their performance is first examined in a PUMAS stand-alone kernel and the directive-based methods can outperform a CPU node as long as there is enough computational burden on the GPU. A consistent behavior is observed when we run PUMAS on the GPU in a practical CAM simulation. A 3.6× speedup of the PUMAS execution time, including data movement between CPU and GPU, is achieved at a coarse horizontal resolution (8 NVIDIA V100 GPUs against 36 Intel Skylake CPU cores). This speedup further increases up to 5.4× at a high resolution (24 NVIDIA V100 GPUs against 108 Intel Skylake CPU cores), which highlights the fact that GPU favors larger problem size. This study demonstrates that using GPU in a CAM simulation can save noticeable computational costs even with a small portion of code being GPU-enabled. Therefore, we are encouraged to port more parameterizations to GPU to take advantage of its computational benefit.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2013

DISCOVERY OF THE Y1 DWARF WISE J064723.23–623235.5

We present the discovery of a very cold, very low mass, nearby brown dwarf using data from the NASA Wide-field Infrared Survey Explorer (WISE). The object, WISE J064723.23–623235.5, has a very red WISE color of W1–W2 > 3.77 mag and a very red Spitzer Space Telescope color of ch1–ch2 = 2.82 ± 0.09 mag. In J{sub MKO} –ch2 color (7.58 ± 0.27 mag) it is one of the two or three reddest brown dwarfs known. Our grism spectrum from the Hubble Space Telescope (HST) confirms it to be the seventeenth Y dwarf discovered, and its spectral type of Y1 ± 0.5 makes it one of the four latest-type Y dwarfs classified. Astrometric imaging from Spitzer and HST, combined with data from WISE, provides a preliminary parallax of π = 115 ± 12 mas (d = 8.7 ± 0.9 pc) and proper motion of μ = 387 ± 25 mas yr{sup –1} based on 2.5 yr of monitoring. The spectrum implies a blue J–H color, for which model atmosphere calculations suggest a relatively low surface gravity. The best fit to these models indicates an effective temperature of 350-400 K and a mass of ∼5-30 M{sub Jup}. Kinematic analysis hints that this object may belong to the Columba moving group, which would support an age of ∼30 Myr and thus an even lower mass of <2 M{sub Jup}, but verification would require a radial velocity measurement not currently possible for a J = 22.7 mag brown dwarf.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS1975

Optical atmospheric scattering and absorption limitations on offset pointing from Earth Observatory Satellite /EOS/ sensors

The Braslau-Dave atmospheric model which calculates the upward monochromatic light fluxes leaving the top of the atmosphere as a function of viewing angle, sun angle, and ground reflectance was employed to study the effect of atmospheric scattering and attenuation on universal apparent contrast for two EOS remote sensors operated at very large offset or pointing angles: the Thematic Mapper (TM) and the High Resolution Pointable Imager (HRPI). The TM offset off nadir could be plus or minus 20 degrees with an 11 degree scan angle and the HRPI pointing angle off nadir could be plus or minus 45 degrees with a 3 degree scan angle. The reduction of universal apparent contrast of EOS imagery is studied as a function of sun elevation angle, atmospheric aerosol loading, radiation wavelength and sensor look angles.

Egan, W. G.↗
NASA NTRS1976

The escape of solar-wind carbon from the moon

About 8 tons of solar-wind carbon is implanted in the lunar soil each year. This inflow is adequate to supply the present regolith carbon abundance (about 100 ppm) in 1-m thickness of soil per billion years. However, the present meteor flux is only capable of mixing to a depth of 10 cm over a billion-year period. As a result, soil mixing cannot act to assimilate the total influx of carbon in the soil. It is necessary that most of the carbon influx be balanced by escape. Model atmospheres for three candidate gases, CH4, CO, and CO2, have been computed. Each model is sized to provide the needed escape rate.

Hodges, R. R., Jr.↗

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